Journal of Environmental Chemical Engineering
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2025
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IF 7.2
Xiteng Yan,Xiaohan Chen,Runping Ye,Jingwen Tao,Gang Feng,Feiyang Hu,Honglin Hu,Claudia Li,Kang Hui Lim,Tao Wen,Yuan Wang,Xinhao Li,Rongbin Zhang,Sibudjing Kawi
Ammonia (NH 3 ) decomposition is a practical approach to overcome the challenges associated with hydrogen storage and transportation. The choice of catalyst and understanding the catalytic mechanism are key factors in optimizing H 2 production by NH 3 decomposition performance. In this work, a series of alkali metal-doped Fe-based catalysts were synthesized via a solvothermal method, and the formation of Fe x N active phases was systematically investigated. The Fe-based catalysts were pretreated under different atmospheres (H 2 , NH 3 , and N 2 ), followed by comprehensive characterization using BET, XRD, SEM, NH 3 -TPD, XPS, and other techniques. The optimized catalytic activity for NH 3 decomposition was attributed to the formation of Fe x N active phases, and the formation pathway of Fe x N active phases and their catalytic promotion mechanism were further elucidated through XRD, NH 3 -TPD-MS, and XPS analyses. Significantly, catalysts treated with pure NH 3 exhibited an increase in the electron density of Fe species and a decrease in the apparent activation energy. The incorporation of alkali metal doping further amplified this effect, ultimately leading to enhanced hydrogen production performance from NH 3 decomposition. This work underscores the critical function of the Fe x N active phase in facilitating efficient NH 3 decomposition for hydrogen generation, offering invaluable insights into the development of sophisticated alkali metal-doped Fe-based catalysts.
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CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Wenhan Zhao,Yingjie Li,Zhiwei Chu,Duo Xu,Kuihua Han,Zirui He
Catalytic methane decomposition (CMD) process has garnered significant attention for CO 2 -free hydrogen production. Fe catalyst has been widely investigated due to its low-cost and environmentally friendly features, but is prone to rapid deactivation due to elevated temperatures and coke deposition. To address these limitations, we synthesized a series of spinel-supported Fe catalysts with varying Fe/Mg/Al ratios via the sol–gel method. These catalysts were evaluated in a fixed-bed reactor, revealing that CMD performance depends significantly on Fe positioning within the spinel lattice in the as-prepared catalysts. Methane conversion was optimal and stable when Fe occupied octahedral sites, achieving 86.7 % CH 4 conversion and 92.9 % H 2 concentration in the outlet gas at 850 °C and 2 L g cat −1 h −1 . The mesoporous spinel structure enhances high-temperature stability and improves coke tolerance, which also contributed to additional layers of multi-walled carbon nanotubes. Density functional theory (DFT) calculations further identified the spinel-supported Fe catalysts as top performers. The energy barriers for the CMD process on Fe/MgAl 2 O 4 (1 1 1) and Fe/MgAl 2 O 4 (1 0 0) were lower than those on Fe(1 1 0). The difference charge density and Bader charge results of CH adsorption and dissociation on the structures, which was the rate-limiting step, demonstrated that the spinel support facilitated the efficient transportation and placement of electrons to the Fe cluster, thereby promoting C–H bond breaking. These findings offer novel insights into the design of cost-effective CMD catalysts with stable catalytic performance and high coke tolerance.
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SENSORS AND ACTUATORS B-CHEMICAL
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2025
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IF 7.7
Jintao Wu,Yanghai Gui,Kuan Tian,Shuaishuai Zhao,Dongjie Guo,Huishi Guo,Xiaoyun Qin,Xiaomei Qin,Yao Guo
As hydrogen is widely used as a clean energy source, the hazards of its flammable and explosive properties are gradually emphasized. Therefore, it is imminent to develop a hydrogen sensor with high response, fast detection speed and low detection limit. In this paper, a PdO/WO 3 composite with fruit-leaf-like structure was synthesized by in-situ hydrothermal and self-assembly impregnation method, and its H 2 sensing performance was investigated. The results show that the self-assembled loading of PdO can greatly improve the H 2 sensing performance of WO 3 , in which the PdO/WO 3 -1 sensor exhibits a very high response value (338.7) and a very short response/recovery time (1 s/4 s) at 120°C to 100 ppm H 2 . The enhanced sensor performance is mainly due to the catalytic effect of the noble metal PdO on H 2 and the synergistic effect between WO 3 and PdO. The growth rhythm of PdO nanoparticles and the effect on the H 2 sensing performance of PdO/WO 3 composites were also explained by varying the concentration of PdCl 2 solution. The density functional theory calculation proves that the hydrogen sensing performance is improved after the combination of PdO and WO 3 . This study provides a feasible solution for the development of high-performance WO 3 -based H 2 sensors.
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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
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2025
·Vol. 36
·期 21
·1-13
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IF 2.8
Zhou Mincong,Li Xu,Zheng Yichen,Wang Qingji
The in-situ growth of sensitive materials has progressively emerged as a prevalent trend. In this paper, SnW 3 O 9 nanosheet arrays are synthesized by aerosol-assisted chemical vapor deposition (AACVD), which is a method for in-situ preparation of sensitive films for gas sensors. Subsequently, Pt-Au is loaded onto the SnW 3 O 9 nanosheet arrays by the wet impregnation process. Ultimately, a H 2 sensor with high selectivity was successfully fabricated. At the optimum operating temperature of 310 °C, the response value of PtAu/SnW 3 O 9 -30 sensor to 100 ppm H 2 is 6.5 times of 100 ppm NH 3 , 7.6 times of 100 ppm CO and 10.1 times of 100 ppm CH 4 . Meanwhile, the sensor performs excellent anti-interference capability under the mixed gases between 100 ppm H 2 and 100 ppm CO, CO 2 and CH 4 , respectively. In addition, the sensor has good stability with different relative humidity. The excellent gas sensing performance of the sensor can primarily be attributed to the unique morphology of SnW 3 O 9 nanosheet arrays and the introduction of Pt-Au. The in-situ growth of PtAu/SnW 3 O 9 nanosheet arrays on planar substrate can be great potential for application in fabricating highly selective H 2 gas sensor.
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SENSORS AND ACTUATORS B-CHEMICAL
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2025
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IF 7.7
Yuxiao Jiang,Kelin Hu,Jing Zhang,Tao He,Bin Yu,Xinyuan Li,Jiarong Yang
This research focused on the synthesis of In 2 O 3 /Ni x O y nanocomposites utilizing the conventional template method. The resulting gas sensor, designed for H 2 detection, demonstrates a sensing behavior that is dependent on temperature. Various characterization techniques were employed to analyze the synthesized In 2 O 3 /NiO composite materials. The results obtained from tests conducted at different temperatures reveal that the sensor maintains a stable n-type response for H 2 at temperatures exceeding 240°C, while exhibiting an atypical p-type response at lower temperatures. This transition in adsorption behavior enables the In 2 O 3 /Ni x O y composites to function as a dual-mode sensor capable of detecting H 2 . The temperature-induced transformation is likely attributable to the interplay of several mechanisms. This article elucidates this phenomenon by examining factors such as activation energy, TGA/DSC, adsorbed oxygen, heterojunction formation, and humidity effects. This study contributes to the understanding of the transformation mechanisms underlying MOS gas sensing behavior.
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APPLIED SURFACE SCIENCE
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2025
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IF 6.9
Junya Wang,Chenxi Ma,Shikun Wen,Ping Ning,Yu Zhang,Yi Liu
This study synthesized a composite material of ZIF-67 and black titanium (BT) with high CO 2 reduction capability via a mechanochemical method. Through in-depth analysis of the morphology, structure, optical properties, and electrochemical behavior of the ZIF-67-BT composite photocatalyst, it was confirmed that the composite successfully formed an S-scheme heterojunction structure. This configuration can effectively separate photogenerated charge carriers, resulting in superior CO 2 reduction performance. The findings indicate that the composite material has optimal catalytic performance when the ZIF-67 doping content reaches 30 wt% (30 %ZIF-BT). Within 5 h, 30 %ZIF-BT exhibited excellent photocatalytic activity, with CO and H 2 yields reaching 2486.4 μmol·g −1 and 3495.0 μmol·g −1 , which were 44.0 and 29.4 times greater than the yields of BT, and 2.4 and 1.4 times than ZIF-67. The syngas (comprising CO and H 2 ) generated by ZIF-BT, with an adjustable CO to H 2 ratio ranging from 1:1.40 to 1:2.47, is regarded as a significantly beneficial and crucial intermediate for further conversion into valuable hydrocarbon fuels via Fischer-Tropsch synthesis. This research offers a feasible method to construct S-scheme heterojunction in ZIF-BT composite materials.
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Surfaces and Interfaces
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2025
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IF 6.3
Ting Li,Jiantao Bi,Huajing Li,Qing Li,Yuangang Li
The synergistic coupling of photocatalytic C C bond construction and H 2 evolution presents a promising strategy for concurrent organic synthesis and sustainable H 2 evolution. Nevertheless, precisely regulating the reaction pathways to enhance the selectivity of target products remains a challenging. Here, the Sv-CdS/TiO 2 Ni 2 P photocatalyst containing sulfur vacancies was synthesized via calcination, achieving highly selective conversion of 4-pyridinemethanol into the C C coupling product 1,2-di-(4-pyridyl)-1,2-ethanediol under visible-light irradiation, with a selectivity of 96.59 %. In comparison, the M-CdS/TiO 2 Ni 2 P photocatalyst prepared by mechanical mixing exhibits superior H 2 evolution activity of 6.48 mmol·g -1 ·h -1 . Mechanism studies reveal that 4-pyridinemethanol interacts with the Sv-CdS/TiO 2 Ni 2 P photocatalyst through the N atom, which preferentially activates the sp 3 C H bond of 4-pyridinemethanol to generate •CH(OH)C 5 H 4 N radical for further C C coupling reaction. This work not only highlights the selective regulation of the 4-pyridinemethanol C C coupling pathway by sulfur vacancies engineering, but also provides new insights for achieving efficient photocatalytic organic synthesis and green H 2 evolution.
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JOURNAL OF THE ENERGY INSTITUTE
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2025
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IF 6.2
Wenzhe Zhang,Shanshan Dai,Yong Liu,Jie Li,Guozhang Chang,Cuiping Wang,Jian Zhang
The utilization of industrially generated lignin is an important aspect of achieving worldwide carbon neutrality. In this study, Ni/CaO, Ce/CaO and (Ni-Ce)/CaO catalysts were prepared using an impregnation method to improve the production of H 2 -enriched syngas from lignin steam gasification. Results show that the Ni/CaO and Ce/CaO exhibited different effects when applied to steam gasification, the former improved the conversion of solid lignin whereas the latter promoted decomposition of the resulting volatiles. The (Ni-Ce)/CaO catalyst provided a remarkable synergistic effect on production of H 2 -enriched syngas. The mass-based yield of gaseous products and the volume-based proportion of H 2 in these products were respectively 70.8% and 61.1% in the presence of the (Ni-Ce)/CaO catalyst with a Ni-to-Ce molar ratio of 1:0.9. The H 2 yields obtained from this material were found to gradually decrease from 763 to 681 mL/(g lignin) during five repeated uses. This gradual deactivation of the (Ni-Ce)/CaO catalyst was ascribed to both carbon deposition and the formation of CaSO 4 by reactions between sulfur in the lignin ash and the CaO component.
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SENSORS AND ACTUATORS B-CHEMICAL
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2025
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IF 7.7
Lin Chen,Xi Chen,Fei Wang,Yu Tong,Kewei Zhang,Zhengbo Han,Mingzhe Zhang
Metal-organic frameworks (MOFs) are regarded as potential candidate materials with great application prospects in the field of gas sensing. In this study, MOF derivatives were anchored onto MXene sheets through self-assembly technology to prepare a heterojunction material ZnO/Ti 3 C 2 T x MXene with high specific surface area, achieving ultrafast dual gas sensing behavior for H 2 /NO 2 . At a low temperature of 80°C, the ZnO/ Ti 3 C 2 T x MXene heterojunction sensor exhibited an ultrafast response (23.17%) to 500 ppb H 2 within 3.2 s. After a moderate temperature increase to 180°C, it also demonstrated significant sensing performance (46.3%) to 500 ppb NO 2 within 4 s. The electronic interaction mechanism of ZnO/ Ti 3 C 2 T x MXene heterostructures in H 2 and NO 2 detection was revealed through density functional theory calculations and in-situ Raman spectroscopy, clarifying the influence of interfacial charge transfer on sensing performance. Heterogeneous structures achieve the regulation of gas adsorption-induced electron rearrangement and carrier modulation by constructing interface charge-regulating channels, significantly enhancing the response rate, selectivity and reversibility in the detection of H 2 and NO 2 , thereby enabling highly sensitive and trace detection of the two gases.
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Industrial Chemistry & Materials
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2025
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IF 11.9
Shenzhen Cong,Si Sun,YiJing Zhang,Ming Wang,Zhehua Jia,Jiaoyu Peng,Huan Pang
Metal-organic framework (MOF) membranes have received widespread research attention as a novel membrane material for H2/CO2 separation. The preparation of MOF membranes can be extended by constructing MOF membranes with homogeneous heterogeneous structure and the MOF membranes with high permeance and high selectivity can be prepared. Here, we use the chelation-assisted interfacial growth process to construct a seeding layer, and then prepare Co-Zn-ZIF-L membranes with homogeneous heterogeneous structure by secondary growth for the efficient separation of H2/CO2. The resulting Co-Zn-ZIF-L membranes show an H2 permeances of 2156 GPU and the H2/CO2 selectivity of 31.6 at 298K and 1.0 bar, surpassing the Robeson upper bond (2008). Furthermore, the Co-Zn-ZIF-L membrane has a H2/CO2 separation stability of 65 h and can efficiently separate to obtain pure H2.
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Chemistry-An Asian Journal
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2024
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IF 3.5
Chunxia Yang,Hailong Cao,Fengyun Su,Mengzhen Tian,Haiquan Xie,Yezhen Zhang,Xiaoli Jin,Xin Li,Zhengdao Li
Photocatalytic H 2 evolution by water splitting is a promising approach to address the challenges of environmental pollution and energy scarcity. Graphitic carbon nitride (g-C 3 N 4 ) has emerged as a star photocatalyst because of its numerous advantages. To address the limitations of traditional g-C 3 N 4 , namely its inadequate visible light response and rapid recombination of photogenerated carriers, we employed a schiff base reaction to synthesize −C=N− doped g-C 3 N 4 . The introduction of −C=N− groups at the bridging nitrogen sites induced structural distortion in g-C 3 N 4 , facilitating n-π* electronic transitions from the lone pair electrons of nitrogen atom and extending light absorption up to 600 nm. Moreover, the presence of heterogeneous π-conjugated electron distribution effectively traps photogenerated electrons and enhances charge carrier separation. Benefiting from its expanded spectral response range, unique electronic properties, increased specific surface area, the doped g-C 3 N 4 exhibited outstanding photocatalytic H 2 evolution performance of 1050.13 μmol/g/h. The value was 5.9 times greater than the pristine g-C 3 N 4 .
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PubMed
高影响因子
Molecular Catalysis
·
2024
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IF 3.9
Jiani Qin,Huannan Wu,Yanli Dong,Fangxin Zhan,Miao Liao,Bao Pan,Chuanyi Wang
The porous semi-coke activated carbon (SAC) was derived from solid waste semi-coke (SC) powder by an activation process. Subsequently, a highly efficient photocatalyst (SAC/CN) was prepared by loading SAC onto carbon nitride (CN). The SAC/CN composite exhibited an increased surface area, well-dispersed layered CN, abundant delocalization electrons, redshift in light absorption, and a more negative conduction band (CB) edge. The optimal 0.7 %SAC/CN 600 sample exhibited the highest H 2 production rate of 12.86 mmol·h −1 ·g −1 , which is 8.0-fold higher than that of pristine CN. The SAC/CN photocatalysts also demonstrated excellent stability and reusability. Photoluminescence (PL) and electrochemical measurements indicated enhanced charge separation/transfer efficiency in the SAC/CN composite. These findings propose a novel approach for recycling of coal chemical solid waste coupled with CN photocatalysts to achieve efficient solar-to-chemical energy conversion.
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